Formation Of Secondary Particulate Matter Research Articles

Predicted and observed changes in summertime biogenic and total organic aerosol in the southeast United States from 2001 to 2010

Biogenic secondary organic aerosol (bSOA) is a major component of atmospheric particulate matter (PM2.5) in the southeast United States especially during the summer, when emissions of biogenic volatile organic compound (VOCs) are high and emissions from anthropogenic sources enhance the formation of secondary particulate matter. In this work we test the hypothesis whether a chemical transport model (PMCAMx) that includes a detailed description of gas-phase chemistry, secondary organic aerosol (SOA) formation based on the volatility basis set (VBS), and interactions among compounds based on partitioning theory can predict organic aerosol (OA) concentrations that are consistent with the observed changes in OA in response to significant changes in anthropogenic emissions during the summers of 2001 and 2010. The model had good performance for OA for both periods and its predictions were consistent with the observed changes in both the urban and rural areas. The fractional error of OA predictions remained practically the same (0.41 and 0.44 at Chemical Speciation Network (CSN) sites and 0.40 to 0.41 at Interagency Monitoring of Protected Visual Environments (IMPROVE) sites in the summers of 2001 and 2010 respectively) in the two examined periods. The fractional bias of OA predictions increased from 0.10 to 0.22 at CSN sites and decreased from 0 to −0.09 at IMPROVE sites between the two periods. Average predicted bSOA concentrations in the southeast US did not change appreciably from the summer of 2001 to the summer of 2010, while the anthropogenic SOA decreased by 45%. As a result, the biogenic fraction of predicted total OA increased from 0.46 in 2001 to 0.63 in 2010. Partitioning effects due to reduced anthropogenic OA from 2001 resulted in 0.4 μg m−3 less biogenic OA on average in the southeast US in the summer of 2010. This was offset by biogenic SOA increases due to higher biogenic vapor emissions in the warmer 2010 summer. Removing the NOx-dependence of SOA formation yields resulted in higher fractional error and fractional bias at both CSN and IMPROVE sites in both summer periods, demonstrating the efficacy of the current formulation of SOA yields. The results of the analysis support the conclusion that a CTM that simulates NOx-dependent SOA chemistry and semivolatile partitioning of SOA material can consistently predict the observed changes in a region rich in biogenic VOCs and SOA.

Air quality and health effects of a transition to ammonia–fueled shipping in Singapore

Ammonia has been proposed to replace heavy fuel oil (HFO) in the shipping industry by 2050. When produced with low-carbon electricity, ammonia can reduce greenhouse gas emissions. However, ammonia emissions also contribute to local air pollution via the formation of secondary particulate matter. We estimate the potential ammonia emissions from storage and bunkering operations for shipping in Singapore, a port that accounts for 20% of global bunker fuel sales, and their impacts on air quality and health. Fuel storage and bunkering can increase total gaseous ammonia emissions in Singapore by up to a factor of four and contribute to a 25%–50% increase in ambient PM2.5 concentration compared to a baseline scenario with HFO, leading to an estimated 210–460 premature mortalities in Singapore (30%–70% higher than the baseline). Proper abatement on storage and bunkering can reduce these emissions and even improve ambient PM2.5 concentrations compared to the baseline. Overall, while an energy transition from HFO to ammonia in the shipping industry could reduce global greenhouse gas and air pollutant burdens, local policies will be important to avoid negative impacts on the communities living near its supply chain.

Key factors for abating particulate matter in a highly industrialized area in N Spain: Fugitive emissions and secondary aerosol precursors

In highly industrialized areas, abating particulate matter (PM) is complex owing to the variety of emission sources with different chemical profiles that may mix in the atmosphere. Gijón—an industrial city in northern Spain—was selected as a case study to better understand the key emission sources and improve air quality in highly industrialized areas. Accordingly, the trends of various air quality indicators (PM10, PM2.5, SO2, NO2, and O3) during the past decade (2010–2019) were analyzed. Additionally, the inorganic and organic PM10 compositions were analyzed for source apportionment studies and to assess the impact of COVID-19 restrictions on PM10 levels.The results revealed that over the past decade, PM10 concentrations decreased, whereas PM2.5 concentrations dominated by secondary inorganic aerosols (SIA) remained relatively constant. Notably, during the COVID-19 lockdown, the PM10 concentration increased by 9.1%, primarily owing to an increase in regional SIA (>65%) due to specific meteorological conditions that favor the formation of secondary PM from gaseous precursors. Overall, eight key PM10 sources were identified: “industrial fugitive PM resuspension” (FPM, 28% of mean PM10 concentration), “aged sea spray” (SSp, 16%), “secondary nitrate” (SN, 15%), “local diffuse source” (LPM, 12%), “solid fuel combustion” (SFC, 7.8%), “biomass burning” (BB, 7.4%), “secondary sulphate” (SSu, 6.0%), and “sinter” (SIN, 4.5%). The PM10 concentration in Gijón is significantly influenced by the integrated steel industry (FPM, SFC, and SIN; 41% of PM10) and fugitive primary PM emissions were the main source (FPM and LPM; 40%). To reduce PM10 and PM2.5 concentrations, industrial fugitive emissions, which are currently poorly regulated, and SIA precursors must be abated.This study provides a methodological approach that combines trend analysis, chemical speciation, and source apportionment for assessing pollution abatement strategies in industrialized areas with a complex mix of emission sources.

An improved representation of fire non-methane organic gases (NMOGs) in models: emissions to reactivity

Abstract. Fires emit a substantial amount of non-methane organic gases (NMOGs), the atmospheric oxidation of which can contribute to ozone and secondary particulate matter formation. However, the abundance and reactivity of these fire NMOGs are uncertain and historically not well constrained. In this work, we expand the representation of fire NMOGs in a global chemical transport model, GEOS-Chem. We update emission factors to Andreae (2019) and the chemical mechanism to include recent aromatic and ethene and ethyne model improvements (Bates et al., 2021; Kwon et al., 2021). We expand the representation of NMOGs by adding lumped furans to the model (including their fire emission and oxidation chemistry) and by adding fire emissions of nine species already included in the model, prioritized for their reactivity using data from the Fire Influence on Regional to Global Environments (FIREX) laboratory studies. Based on quantified emissions factors, we estimate that our improved representation captures 72 % of emitted, identified NMOG carbon mass and 49 % of OH reactivity from savanna and temperate forest fires, a substantial increase from the standard model (49 % of mass, 28 % of OH reactivity). We evaluate fire NMOGs in our model with observations from the Amazon Tall Tower Observatory (ATTO) in Brazil, Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) and DC3 in the US, and Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) in boreal Canada. We show that NMOGs, including furan, are well simulated in the eastern US with some underestimates in the western US and that adding fire emissions improves our ability to simulate ethene in boreal Canada. We estimate that fires provide 15 % of annual mean simulated surface OH reactivity globally, as well as more than 75 % over fire source regions. Over continental regions about half of this simulated fire reactivity comes from NMOG species. We find that furans and ethene are important globally for reactivity, while phenol is more important at a local level in the boreal regions. This is the first global estimate of the impact of fire on atmospheric reactivity.

Does Ambient Secondary Conversion or the Prolonged Fast Conversion in Combustion Plumes Cause Severe PM2.5 Air Pollution in China?

The ambient formation of secondary particulate matter (ambient FSPM) is commonly recognized as the major cause of severe PM2.5 air pollution in China. We present observational evidence showing that the ambient FSPM was too weak to yield a detectable contribution to extreme PM2.5 pollution events that swept northern China between 11 and 14 January 2019. Although the Community Multiscale Air Quality (CMAQ) model (v5.2) reasonably reproduced the observations in January 2019, it largely underestimated the concentrations of the PM2.5 during the episode. We propose a novel mechanism, called the “in-fresh-stack-plume non-precipitation-cloud processing of aerosols” followed by the evaporation of semi-volatile components from the aerosols, to generate PM2.5 at extremely high concentrations because of highly concentrated gaseous precursors and large amounts of water droplets in fresh cooling combustion plumes under poor dispersion conditions, low ambient temperature, and high relative humidity. The recorded non-precipitation-cloud processing of the aerosols in fresh stack combustion plumes normally lasts 20–30 s, but it prolongs as long as 2–5 min under cold, humid, and stagnant meteorological conditions and expectedly causes severe PM2.5 pollution events. Regardless of the presence of the natural cloud in the planetary boundary layer during the extreme events, the fast conversion of air pollutants in water droplets and the generation of the PM2.5 through the non-precipitation-cloud processing of aerosols always occur in fresh combustion plumes. The processing of aerosols is detectable using a nano-scan particle sizer assembled on an unmanned aerial vehicle to monitor the particle formation in stack plumes. In-fresh-stack-plume processed aerosols under varying meteorological conditions need to be studied urgently.

Measurements of nitrous oxide and ammonia emissions from diesel automobile under the real-world driving conditions using laser absorption spectrometer

Nitrous oxide (N2O) is a greenhouse gas and contributes to ozone depletion, and ammonia (NH3) contributes to the formation of secondary particulate matter. To reduce global warming and particulate matter, the real-world levels of N2O and NH3 emitted from automobiles is required to be examined. However, there are a few studies on the measurements of N2O and NH3 in automobile exhaust under the real-world conditions. In this study, we have measured the real-world emissions of N2O and NH3 from the latest diesel vehicle equipped with an urea-SCR system. N2O was measured by an on-board system using mid-IR laser spectroscopy and NH3 was measured using a sensor-based measurement technique. As a result, NH3 was not emitted, while N2O was emitted intermittently when vehicle was running.

Reactive nitrogen compounds and their influence on human health: an overview.

Nitrogen (N)is a critical component of food security, economy and planetary health. Human production of reactive nitrogen (Nr) via Haber-Bosch process and cultivation-induced biological N2 fixation (BNF) has doubled global N cycling over the last century. The most important beneficial effect of Nr is augmenting global food supplies due to increased crop yields. However, increased circulation of Nr in the environment is responsible for serious human health effects such as methemoglobinemia ("blue baby syndrome") and eutrophication of coastal andinland waters. Furthermore, ammonia (NH3) emission mainly from farming and animal husbandary impacts not only human health causing chronic lung disease, inflammation of human airways and irritation of eyes, sinuses and skin but is also involved in the formation of secondary particulate matter (PM) that plays a critical role in environment and human health. Nr also affects human health via global warming, depletion of stratospheric ozone layer resulting in greater intensity of ultra violet B rays (UVB) on the Earth's surface, and creation of ground-level ozone (through reaction of NO2 with O2). The consequential indirect human health effects of Nr include the spread of vector-borne pathogens, increased incidence of skin cancer, development of cataracts, and serious respiratory diseases, besides land degradation. Evidently, the strategies to reduce Nr and mitigate adverse environmental and human health impacts include plugging pathways of nitrogen transport and loss through runoff, leaching and emissions of NH3, nitrogen oxides (NO x ), and other N compounds; improving fertilizer N use efficiency; reducing regional disparity in access to N fertilizers; enhancing BNF to decrease dependence on chemical fertilizers; replacing animal-based proteins with plant-based proteins; adopting improved methods of livestock raising and manure management; reducing air pollution and secondary PM formation; and subjecting industrial and vehicular NO x emission to pollution control laws. Strategic implementation of all these presents a major challenge across the fields of agriculture, ecology and public health. Recent observations on the reduction of air pollution in the COVID-19 lockdown period in several world regions provide an insight into the achievability of long-term air quality improvement. In this review, we focus on complex relationships between Nr and human health, highlighting a wide range of beneficial and detrimental effects.

NO2 levels as a contributing factor to COVID-19 deaths: The first empirical estimate of threshold values

This study represents the first empirical estimation of threshold values between nitrogen dioxide (NO2) concentrations and COVID-19-related deaths in France. The concentration of NO2 linked to COVID-19-related deaths in three major French cities were determined using Artificial Neural Networks experiments and a Causal Direction from Dependency (D2C) algorithm. The aim of the study was to evaluate the potential effects of NO2 in spreading the epidemic. The underlying hypothesis is that NO2, as a precursor to secondary particulate matter formation, can foster COVID-19 and make the respiratory system more susceptible to this infection. Three different neural networks for the cities of Paris, Lyon and Marseille were built in this work, followed by the application of an innovative tool of cutting the signal from the inputs to the selected target. The results show that the threshold levels of NO2 connected to COVID-19 range between 15.8 μg/m3 for Lyon, 21.8 μg/m3 for Marseille and 22.9 μg/m3 for Paris, which were significantly lower than the average annual concentration limit of 40 μg/m³ imposed by Directive 2008/50/EC of the European Parliament.

Describing the trend of ammonia, particulate matter and nitrogen oxides: The role of livestock activities in northern Italy during Covid-19 quarantine

Nitrogen oxides (NOx), sulphur oxides (SOx) and ammonia (NH3) are among the main contributors to the formation of secondary particulate matter (PM2.5), which represent a severe risk to human health. Even if important improvements have been achieved worldwide, traffic, industrial activities, and the energy sector are mostly responsible for NOx and SOx release; instead, the agricultural sector is mainly responsible for NH3 emissions.Due to the emergency of coronavirus disease, in Italy schools and universities have been locked down from late February 2020, followed in March by almost all production and industrial activities as well as road transport, except for the agricultural ones. This study aims to analyze NH3, PM2.5 and NOx emissions in principal livestock provinces in the Lombardy region (Brescia, Cremona, Lodi, and Mantua) to evaluate if and how air emissions have changed during this quarantine period respect to 2016–2019. For each province, meteorological and air quality data were collected from the database of the Regional Agency for the Protection of the Environment, considering both data stations located in the city and the countryside. In the 2020 selected period, PM2.5 reduction was higher compared to the previous years, especially in February and March. Respect to February, PM2.5 released in March in the city stations reduced by 19%–32% in 2016–2019 and by 21%–41% in 2020. Similarly, NOx data of 2020 were lower than in the 2016–2019 period (reduction in March respect to February of 22–42% for 2016–2019 and of 43–62% for 2020); in particular, this can be observed in city stations, because of the current reduction in anthropogenic emissions related to traffic and industrial activities. A different trend with no reductions was observed for NH3 emissions, as agricultural activities have not stopped during the lockdown. Air quality is affected by many variables, for which making conclusions requires a holistic perspective. Therefore, all sectors must play a role to contribute to the reduction of harmful pollutants.

The impact of ship emissions on air quality and human health in the Gothenburg area – Part 1: 2012 emissions

Abstract. Ship emissions in and around ports are of interest for urban air quality management in many harbour cities. We investigated the impact of regional and local ship emissions on urban air quality for 2012 conditions in the city of Gothenburg, Sweden, the largest cargo port in Scandinavia. In order to assess the effects of ship emissions, a coupled regional- and local-scale model system has been set up using ship emissions in the Baltic Sea and the North Sea as well as in and around the port of Gothenburg. Ship emissions were calculated with the Ship Traffic Emission Assessment Model (STEAM), taking into account individual vessel characteristics and vessel activity data. The calculated contributions from local and regional shipping to local air pollution in Gothenburg were found to be substantial, especially in areas around the city ports. The relative contribution from local shipping to annual mean NO2 concentrations was 14 % as the model domain average, while the relative contribution from regional shipping in the North Sea and the Baltic Sea was 26 %. In an area close to the city terminals, the contribution of NO2 from local shipping (33 %) was higher than that of road traffic (28 %), which indicates the importance of controlling local shipping emissions. Local shipping emissions of NOx led to a decrease in the summer mean O3 levels in the city by 0.5 ppb (∼2 %) on average. Regional shipping led to a slight increase in O3 concentrations; however, the overall effect of regional and the local shipping together was a small decrease in the summer mean O3 concentrations in the city. In addition, volatile organic compound (VOC) emissions from local shipping compensate up to 4 ppb of the decrease in summer O3 concentrations due to the NO titration effect. For particulate matter with a median aerodynamic diameter less than or equal to 2.5 µm (PM2.5), local ship emissions contributed only 3 % to the annual mean in the model domain, while regional shipping under 2012 conditions was a larger contributor, with an annual mean contribution of 11 % of the city domain average. Based on the modelled local and regional shipping contributions, the health effects of PM2.5, NO2 and ozone were assessed using the ALPHA-RiskPoll (ARP) model. An effect of the shipping-associated PM2.5 exposure in the modelled area was a mean decrease in the life expectancy by 0.015 years per person. The relative contribution of local shipping to the impact of total PM2.5 was 2.2 %, which can be compared to the 5.3 % contribution from local road traffic. The relative contribution of the regional shipping was 10.3 %. The mortalities due to the exposure to NO2 associated with shipping were calculated to be 2.6 premature deaths yr−1. The relative contribution of local and regional shipping to the total exposure to NO2 in the reference simulation was 14 % and 21 %, respectively. The shipping-related ozone exposures were due to the NO titration effect leading to a negative number of premature deaths. Our study shows that overall health impacts of regional shipping can be more significant than those of local shipping, emphasizing that abatement policy options on city-scale air pollution require close cooperation across governance levels. Our findings indicate that the strengthened Sulphur Emission Control Areas (SECAs) fuel sulphur limit from 1 % to 0.1 % in 2015, leading to a strong decrease in the formation of secondary particulate matter on a regional scale was an important step in improving the air quality in the city.

Enhanced secondary pollution offset reduction of primary emissions during COVID-19 lockdown in China.

To control the spread of the 2019 novel coronavirus (COVID-19), China imposed nationwide restrictions on the movement of its population (lockdown) after the Chinese New Year of 2020, leading to large reductions in economic activities and associated emissions. Despite such large decreases in primary pollution, there were nonetheless several periods of heavy haze pollution in eastern China, raising questions about the well-established relationship between human activities and air quality. Here, using comprehensive measurements and modeling, we show that the haze during the COVID lockdown was driven by enhancements of secondary pollution. In particular, large decreases in NOx emissions from transportation increased ozone and nighttime NO3 radical formation, and these increases in atmospheric oxidizing capacity in turn facilitated the formation of secondary particulate matter. Our results, afforded by the tragic natural experiment of the COVID-19 pandemic, indicate that haze mitigation depends upon a coordinated and balanced strategy for controlling multiple pollutants.

A Study on Particulate Matter Footprint Calculation on Transportation Modes

Objective : In this study, we proposed the concept of the particulate matter footprint (PM Footprint) and assessed the PM Footprint in transportation modes (road, rail, and water transportation). In addition, we assessed the contribution of secondary particulate matter formation gas emissions, which contribute to particulate matter formation.Method : To calculate the PM Footprint in the transportation sector, the ReCiPe life cycle impact assessment method in life cycle assessment (LCA) was used. For the PM Footprint of each transportation mode, the life cycle inventory data were multiplied by the characterization factors of PM<sub>10</sub>, PM<sub>2.5</sub> and secondary particulate matter formation emissions such as NOx, SOx, NH<sub>3</sub>. The PM Footprint values were shown in kg PM<sub>2.5</sub> eqv. value.Results and Discussion : The road transportation (trucks) had a much higher PM Footprint value than rail and water transportation in tkm unit based. In the road transportation mode, small size truck such as 3.5 tons (1.37E-03 kg PM<sub>2.5</sub> eqv./tkm), 3.51~5 tons (9.65E-04 kg PM<sub>2.5</sub> eqv./tkm), 1.25 tons (8.38E-04 kg PM<sub>2.5</sub> eqv./tkm), and 1 ton (7.83E-04 kg PM<sub>2.5</sub> eqv./tkm) had higher PM Footprint value than big size trucks. In the rail transportation mode, the diesel rail transportation had the highest PM Footprint value, followed by electric + diesel rail transportation and electric rail transportation. In the water transportation mode, the tanker LNG_100 dwt had the highest PM Footprint value, followed by ro-ro ship coastal, and tanker coastal 500~20,000 dwt. The secondary particulate matter formation emissions (NOx, SOx, NH<sub>3</sub>) contributed to PM Footprint value with 59% in road transportation, 80% in rail transportation, and 61% in water transportation. Conclusions : The PM Footprint values, which shown in this study and the results of the directed polluted PM and secondary gas emissions should be considered for national PM reduction policy and planning. Finally, a certification system using the PM Footprint in this study should be developed and settled down for national PM reduction.

New positive feedback mechanism between boundary layer meteorology and secondary aerosol formation during severe haze events

Severe haze events during which particulate matter (PM) increases quickly from tens to hundreds of microgram per cubic meter in 1–2 days frequently occur in China. Although it has been known that PM is influenced by complex interplays among emissions, meteorology, and physical and chemical processes, specific mechanisms remain elusive. Here, a new positive feedback mechanism between planetary boundary layer (PBL), relative humidity (RH), and secondary PM (SPM) formation is proposed based on a comprehensive field experiment and model simulation. The decreased PBL associated with increased PM increases RH by weakening the vertical transport of water vapor; the increased RH in turn enhances the SPM formation through heterogeneous aqueous reactions, which further enhances PM, weakens solar radiation, and decreases PBL height. This positive feedback, together with the PM-Radiation-PBL feedback, constitutes a key mechanism that links PM, radiation, PBL properties (e.g. PBL height and RH), and SPM formation, This mechanism is self-amplifying, leading to faster PM production, accumulation, and more severe haze pollution.

Ice Nucleation Activity of Graphene and Graphene Oxides.

Aerosols can act as cloud condensation nuclei and/or ice-nucleating particles (INPs), influencing cloud properties. In particular, INPs show a variety of different and complex mechanisms when interacting with water during the freezing process. To gain a fundamental understanding of the heterogeneous freezing mechanisms, studies with proxies for atmospheric INPs must be performed. Graphene and its derivatives offer suitable model systems for soot particles, which are ubiquitous aerosols in the atmosphere. In this work, we present an investigation of the ice nucleation activity (INA) of different types of graphene and graphene oxides. Immersion droplet freezing experiments as well as additional analytical analyses, such as X-ray photoelectron spectroscopy, Raman spectroscopy, and transmission electron microscopy, were performed. We show within a group of samples that a highly ordered graphene lattice (Raman G band intensity >50%) can support ice nucleation more effectively than a lowly ordered graphene lattice (Raman G band intensity <20%). Ammonia-functionalized graphene revealed the highest INA of all samples. Atmospheric ammonia is known to play a primary role in the formation of secondary particulate matter, forming ammonium-containing aerosols. The influence of functionalization on interactions between the particle interface and water molecules, as well as on hydrophobicity and agglomeration processes, is discussed.

Impacts of traffic emissions on atmospheric particulate nitrate and organics at a downwind site on the periphery of Guangzhou, China

Abstract. Particulate matter (PM) pollution on the peripheries of Chinese megacities can be as serious as in cities themselves. Given the substantial vehicular emissions in inner-city areas, the direct transport of primary PM (e.g., black carbon and primary organics) and effective formation of secondary PM from precursors (e.g., NOx and volatile organic compounds) can contribute to PM pollution in buffer zones between cities. To investigate how traffic emissions in inner-city areas impact these adjacent buffer zones, a suite of real-time instruments were deployed in Panyu, downwind from central Guangzhou, from November to December 2014. Nitrate mass fraction was higher on high-PM days, with the average nitrate-to-sulfate ratio increasing from around 0.35 to 1.5 as the PM mass concentration increased from 10 to 160 µg m−3. Particulate nitrate was strongly correlated with excess ammonium (([NH4+] ∕ [SO42−] − 1.5) × [SO42−]), with higher concentrations in December than in November due to lower temperatures. The organic mass fraction was the highest across all PM1 levels throughout the campaign. While organic aerosols (OA) were dominated by secondary organic aerosols (SOA = semi-volatile oxygenated organic aerosols + low-volatility oxygenated organic aerosols) as a campaign average, freshly emitted hydrocarbon-like organic aerosols (HOA) contributed up to 40 % of OA during high-OA periods, which typically occurred at nighttime and contributed 23.8 to 28.4 % on average. This was due to daytime traffic restrictions on heavy-duty vehicles in Guangzhou, and HOA almost increased linearly with total OA concentration. SOA increased as odd oxygen (Ox = O3 + NO2) increased during the day due to photochemistry. A combination of nighttime traffic emissions and daytime photochemistry contributed to the buildup of PM in Panyu. The mitigation of PM pollution in inner-city areas by reducing vehicular traffic can potentially improve air quality in peripheral areas.

Directional passive ambient air monitoring of ammonia for fugitive source attribution; a field trial with wind tunnel characteristics

Atmospheric ammonia is a precursor for secondary particulate matter formation, which harms human health and contributes to acidification and eutrophication. Under the 2012 Gothenburg Protocol, 2005 emissions must be cut by 6% by 2020. In the UK, 83% of total emissions originate from agricultural practices such as fertilizer use and rearing of livestock, with emissions that are spatially extensive and variable in nature. Such fugitive emissions make resolving and tracking of individual site performance challenging. The Directional Passive Air quality Sampler (DPAS) was trialled at Whim Bog, an experimental site with a wind-controlled artificial release of ammonia, in combination with CEH-developed ammonia samplers. Whilst saturation issues were identified, two DPAS-MANDE (Mini Annular Denuder) systems, when deployed in parallel, displayed an average relative deviation of 15% (2–54%) across all 12 directions, with the directions exposed to the ammonia source showing ∼5% difference. The DPAS-MANDE has shown great potential for directional discrimination and can contribute to the understanding and management of fugitive ammonia sources from intensive agriculture sites.

Particulate matter formation from photochemical degradation of organophosphorus pesticides

Several experiments were performed in the European Photo-reactor - EUPHORE - for studying aerosol formation from organophosphorus pesticides such as diazinon, chlorpyrifos, chlorpyrifos-methyl and pirimiphos-methyl. The mass concentration yields obtained (Y) were in the range 5 - 44% for the photo-oxidation reactions in the presence and the absence of NOx. These results confirm the importance of studying pesticides as significant precursors of atmospheric particulate matter due to the serious risks associated to them.The studies based on the use of EUPHORE photoreactor provide useful data about atmospheric degradation processes of organophosphorus pesticides to the atmosphere. Knowledge of the specific degradation products, including the formation of secondary particulate matter, could complete the assessment of their potential impact, since the formation of those degradation products plays a significant role in the atmospheric chemistry, global climate change, radiative force, and are related to health effects.

Plume-in-grid model for the evaluation of particulate matter contribution of industrial point and volume sources: application to refinery sources in the Paris region

To assess the potential contributions of refineries to air pollution requires taking into account the formation of secondary pollutants, such as particulate matter (PM), resulting from the oxidation of emitted precursors. A plume-in-grid (PinG) model is best suited to address this issue, because it provides a realistic representation of the dispersion and transformations of the pollutants in the refinery plumes as they travel from the near field to long-range downwind distances. A PinG model that treats stack emissions as point sources and fugitive emissions as volume sources is applied here to a refinery in the Greater Paris region. The formation of secondary PM in the refinery plumes and the effect of hypothetical refinery emission controls on downwind PM concentrations are investigated. The simulation results emphasise the nonlinear relationships between emission levels and secondary PM species. These results imply that PinG modelling is recommended to correctly assess the potential impacts of refinery emissions on air pollution.

Elucidating severe urban haze formation in China.

As the world's second largest economy, China has experienced severe haze pollution, with fine particulate matter (PM) recently reaching unprecedentedly high levels across many cities, and an understanding of the PM formation mechanism is critical in the development of efficient mediation policies to minimize its regional to global impacts. We demonstrate a periodic cycle of PM episodes in Beijing that is governed by meteorological conditions and characterized by two distinct aerosol formation processes of nucleation and growth, but with a small contribution from primary emissions and regional transport of particles. Nucleation consistently precedes a polluted period, producing a high number concentration of nano-sized particles under clean conditions. Accumulation of the particle mass concentration exceeding several hundred micrograms per cubic meter is accompanied by a continuous size growth from the nucleation-mode particles over multiple days to yield numerous larger particles, distinctive from the aerosol formation typically observed in other regions worldwide. The particle compositions in Beijing, on the other hand, exhibit a similarity to those commonly measured in many global areas, consistent with the chemical constituents dominated by secondary aerosol formation. Our results highlight that regulatory controls of gaseous emissions for volatile organic compounds and nitrogen oxides from local transportation and sulfur dioxide from regional industrial sources represent the key steps to reduce the urban PM level in China.

Fine Atmospheric Particles from Agricultural Practices in Flanders: From Emissions to Health Effects and Limit Values

Agriculture can influence air quality via emissions of ammonia, soil dust and soot. These can be emitted into the atmosphere during farming practices, and contribute in different amounts to the total emissions and concentrations of air particulate matter (PM). The exact contribution of Flemish agricultural emissions to total air PM concentrations and to negative health effects are not well known. In this paper, agricultural emissions in Flanders and the processes leading to secondary PM are reviewed, together with their associated health effects. Agricultural ammonia emissions are a major contributor to local formation of secondary PM, and can increase above normal levels during some smog episodes. From a health perspective, secondary PM formed by ammonia is considered less important. Epidemiological studies suggest that combustion-related particles are the cause of negative health effects, although a reduction in ammonia emissions would reduce acidification and eutrophication of ecosystems. The World Health Organization currently considers PM2.5 as the best indicator for assessing human health effects. Setting an additional limit value for combustion-related particles would target potentially more harmful particles.